dissertation - uni- prozesse sind jedoch weitestgehend noch nicht erforscht. in dieser dissertation

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  • Dissertation

    to be awarded the degree of Doctor rerum naturalium (Dr. rer. nat.) at the

    Faculty of Biology, Chemistry and Earth Science, University of Bayreuth

    submitted by

    M. Sc. Carolin Fürst

    From Schwäbisch Hall

    Bayreuth 2016

    KINETIC STUDIES OF LYOTROPIC

    STRUCTURE FORMATION WITH

    MICROFLUIDICS AND SMALL ANGLE X-

    RAY SCATTERING

  • Die vorliegende Arbeit wurde in der Zeit von Januar 2012 bis Juli 2016 in Bayreuth am

    Lehrstuhl der Physikalischen Chemie unter Betreuung von Herrn Professor Dr. Stephan

    Förster angefertigt.

    Vollständiger Abdruck der von der Fakultät für Biologie, Chemie und Geowissenschaften

    der Universität Bayreuth genehmigten Dissertation zur Erlangung des akademischen

    Grades eines Doktors der Naturwissenschaften (Dr. rer. nat.).

    Dissertation eingereicht am 29.07.2016

    Zulassung durch die Promotionskommission 22.08.2016

    Wissenschaftliches Kolloquium am 02.12.2016

    Amtierender Dekan: Prof. Dr. Stefan Schuster

    Prüfungsausschuss:

    Prof. Dr. Stephan Förster (Erstgutachter)

    Prof. Dr. Jürgen Senker (Zweitgutachter)

    Prof. Dr. Peter Strohriegl (Vorsitz)

    JProf. Dr. Markus Retsch

  • Table of contents

    I

    Summary ............................................................................................................ IV

    Zusammenfassung ........................................................................................... VII

    1 Introduction and Motivation ....................................................................................... 1

    2 Fundamentals ............................................................................................................... 4

    2.1 Mesoscale Materials ............................................................................................... 4

    2.1.1 Amphiphiles ............................................................................................................... 4

    2.1.2 Self-assembly ............................................................................................................. 6

    2.1.2.1 Calculation of Self-assembled Structures ............................................................... 8

    2.1.2.2 Lyotropic Phases .................................................................................................. 11

    2.1.3 Structural Hierarchies ............................................................................................... 14

    2.2 Microfluidics ......................................................................................................... 15

    2.2.1 Motion of Fluids ....................................................................................................... 16

    2.2.1.1 The Navier-Stokes Equation ................................................................................. 17

    2.2.1.2 No-slip Boundary Condition ................................................................................ 23

    2.2.1.3 Pressure Driven Flow .......................................................................................... 24

    2.2.1.4 The Reynolds Number .......................................................................................... 30

    2.2.1.5 Diffusion and Convection ..................................................................................... 31

    2.2.1.6 Péclet Number and Taylor Dispersion ................................................................. 36

    2.2.2 Device Fabrication ................................................................................................... 38

    2.2.2.1 Soft Lithography ................................................................................................... 39

    2.2.2.2 Hot Embossing ..................................................................................................... 41

    2.2.2.3 Rapid Prototyping ................................................................................................ 41

    2.3 Small Angle X-ray Scattering ............................................................................... 43

    2.3.1 Physical Fundamentals of Small Angle X-ray Scattering ........................................ 43

    2.3.2 The Correlation Function ......................................................................................... 51

    2.3.3 Form Factor .............................................................................................................. 53

    2.3.4 Structure Factor ........................................................................................................ 55

    2.3.5 Analyzation of Measured Scattering Patterns .......................................................... 55

    2.3.6 Experimental Set-up ................................................................................................. 60

    2.4 Further Characterization Methods ........................................................................ 62

    2.4.1 Confocal Laser Scanning Microscopy (CLSM) ....................................................... 63

    2.4.2 Cryogenic Transmission Electron Microscopy (Cryo-TEM) ................................... 65

    3 Experiments ................................................................................................................ 69

    3.1 Small Angle X-ray Scattering ............................................................................... 69

    3.2 Confocal Laser Scanning Microscopy .................................................................. 69

    3.3 Cryogenic Transmission Electron Microscopy ..................................................... 69

    3.4 COMSOL Multiphysics ........................................................................................ 70

    4 Results and Discussion ............................................................................................... 71

    4.1 Materials for Microfluidic Devices ....................................................................... 71

    4.1.1 Solvent Resistant Chip Materials ............................................................................. 71

  • Table of contents

    II

    4.1.2 Optical Properties of Chip Materials ........................................................................ 75

    4.1.3 Microfluidic Device Design ..................................................................................... 79

    4.2 Vesicle Formation Pathways Under Very Fast and Very Slow Formation

    Conditions ........................................................................................................................ 81

    4.2.1 Introduction .............................................................................................................. 81

    4.2.2 Materials and Methods ............................................................................................. 83

    4.2.3 Results and Discussion ............................................................................................. 86

    4.2.4 Conclusions ............................................................................................................ 106

    4.3 Solvent Resistant Microfluidic-Hybrid-Chip for Three-Dimensional

    Hydrodynamic Flow Focusing ....................................................................................... 107

    4.3.1 Introduction ............................................................................................................ 107

    4.3.2 Results and Discussion ........................................................................................... 108

    4.3.2.1 Flow and Device Design .................................................................................... 108

    4.3.2.2 Device Fabrication ............................................................................................. 110

    4.3.2.3 Flow Control ...................................................................................................... 111

    4.3.2.4 Application ......................................................................................................... 113

    4.3.3 Experimental .......................................................................................................... 115

    4.3.4 Conclusion .............................................................................................................. 116

    4.4 Self-assembly of Block Copolymers via Micellar Intermediate States into

    Vesicles on Time Scales from Milliseconds to Days..................................................... 118

    4.4.1 Introduction ............................................................................................................ 118

    4.4.2 Materials and Methods ........................................................................................... 120

    4.4.3 Results and Discussion ........................................................................................... 123

    4.4.3.1 Experiments in a 2D-Polyimide Microfluidic Device ........................................ 123

    4.4.3.2 Experiments in SIFEL Microfluidic Device ....................................................... 128

    4.4.3.3 Determination of the Mixing Point ..................................................................... 1

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